He began his academic career, which would occupy the rest of his life, in 1948, teaching at Magdalen College, St. Antony's College (where he created and directed the college's Middle East Centre), the American University of Beirut, the University of Chicago, the University of Pennsylvania, and Harvard. He ended his academic career as Fellow of St. Antony's College and Reader in the History of the Modern Middle East at Oxford. Hourani trained more academic historians of the modern Middle East than any other university historian of his generation. Today his students can be found on the faculties of LSE, Oxford, Cambridge, Harvard, Yale, University of Pennsylvania, Columbia, MIT and the University of Haifa, among others.

Hourani's most popular work is A History of the Arab Peoples (1991), a readable introduction to the history of the Middle East and an international best seller. Arabic Thought in the Liberal Age 1789-1939 (1962) is one of the first scientific attempts at a comprehensive analysis of the nahda, the Arab revival of the nineteenth century, and the opening of the Arab world to modern European culture, and remains one of the major works on this subject. Syria and Lebanon (1946) and Minorities in the Arab World (1947) are other major works. He also wrote extensive works on the orientalist perspective on Middle Eastern cultures through the 18th and 19th centuries, and he developed the influential concept of the "urban notables"—political and social elites in provincial Middle Eastern cities and towns that served as intermediaries between imperial capitals (such as Istanbul under the Ottoman Turks) and provincial society.

Hourani married Christine Mary Odile Wegg-Prosser in 1955, while teaching at Magdalen College, Oxford. He died in Oxford at the age of 77. Mrs. Odile Hourani (b. 1914) died in 2003, shortly after the tenth anniversary of her husband's death. They are both buried at Wolvercote Cemetery in Oxford. Their daughter, Prof. Susanna Hourani, survives them. She is Professor of Pharmacology and Head of Department in the School of Biomedical and Molecular Sciences of the University of Surrey, UK.